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    Magnetoelastic coupling across competing ferromagnetic and ferrimagnetic orders in A-site-disordered NdSmNiMnO6

    John M. Attah-Baah1,2,3, Cledson dos Santos4, Romualdo S. Silva, Jr.5, Maria H. Carvalho6, Raí F. Jucá7, Marcos V. S. Rezende1, Edson C. Passamani4, Roger D. Johnson8,9,10, and Nilson S. Ferreira1,*

    • *Contact author: nilson@academico.ufs.br

    Phys. Rev. B 114, 094408 – Published 4 August, 2026

    DOI: https://doi.org/10.1103/qjn8-rfhl

    Abstract

    We show that the magnetic ground state of the double perovskite NdSmNiMnO6 is jointly controlled by A-site (Nd/Sm) mixing, B-site (Ni/Mn) ordering, and spin-lattice coupling, with the rare-earth sublattice actively participating in the low-energy magnetic balance. Synchrotron x-ray diffraction (SXRD) and Rietveld refinement establish a monoclinic (P21/n) structure with predominant B-site rocksalt order and measurable antisite disorder, while x-ray absorption near-edge structure identifies Ni2+ and Mn4+ valence states. Magnetometry reveals a ferromagnetic (FM) transition at TC≈175K driven by Ni2+-O-Mn4+ exchange, followed at lower temperature by a ferrimagneticlike (FiM) regime when the 3d and 4f sublattices are magnetically ordered. Concomitantly, Raman modes exhibit anomalous hardening below TC and the refined SXRD lattice parameters display clear anomalies at the magnetic transitions, evidencing pronounced magnetoelastic coupling. Spin-polarized density functional theory captures this competition, yielding nearly degenerate FiM and FM solutions (ΔE≈2meV per 20-atom cell) and indicating that coupling of the rare-earth sublattice to the Ni-O-Mn network sets the energy balance. The ferrimagnetic solution carries local moments of ∼1.6 μB on Ni and ∼3.0 μB on Mn and remains insulating, with a gap of 1.6–1.7 eV. With spin-orbit coupling (SOC), the projected Sm3+ spin moment is strongly reduced (4.93 to 0.3 μB), reflecting SOC-driven quenching of the Sm spin polarization, while the gap is nearly unchanged, indicating that the electronic structure is primarily stabilized by Ni/Mn 3d–O 2p hybridization. Our results provide a quantitative framework to disentangle rare-earth A-site magnetism from Ni-O-Mn exchange and to rationalize magnetoelastic responses in A-site-disordered double perovskites near competing magnetic states.

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